The work aims to prepare anthocyanin gelatin/polyvinyl alcohol starch bilayer composite film, so as to improve the comprehensive performance of anthocyanin monolayer film. Six kinds of anthocyanin gelatin/polyvinyl alcohol starch bilayer composite films were prepared by layer-by-layer stretch film technology with purple potato, purple cabbage, black rice, black wolfberry, rose and roselle. Then, the microstructure, moisture content, mechanical properties and optical properties of these films were compared and studied. From the infrared spectroscopy, the molecular structure of the material in the bilayer composite film was mainly the intermolecular force, and no new structure was generated. Except the purple cabbage gelatin/polyvinyl alcohol starch bilayer composite film, the other composite films hadobvious delamination boundary, but the film structure at the junction of the two layers was uniform and compact, with good binding effect. The moisture content of different bilayer films was significantly different, while the moisture content of bilayer composite film was significantly lower than that of anthocyanin monolayer film. There was no significant difference in tensile strength and elongation at break among different bilayer films. Compared with the monolayer anthocyanin gelatin composite film, the tensile strength and elongation at break of the bilayer composite film greatly increased, among which the tensile strength increased by 75% and elongation at break of the purple potato bilayer film increased by 22.9%. The light transmittance of all the bilayer composite films hadlittle difference, all of which were above 80%. The haze of bilayer film increased by about 20% compared with anthocyanin gelatin monolayer film. The prepared bilayer film improves the mechanical properties of monolayer film and enhances the comprehensive properties of anthocyanin gelatin monolayer film.